Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4−

Abstract

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Document Details

Document Type
Pub Defense Publication
Publication Date
Mar 26, 2018
Source ID
10.1063/1.5021185

Entities

People

  • Donald Truhlar
  • Laura Gagliardi
  • Prachi Sharma

Organizations

  • United States Air Force
  • University of Minnesota Supercomputing Institute

Tags

Fields of Study

  • Physics

Readers

  • Quantum Chemistry
  • Quantum spin resonance or Electron Paramagnetic Resonance spectroscopy.

Technology Areas

  • Microelectronics
  • Quantum Computing
  • Space